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Impact of an improved WRF urban canopy model on diurnal air temperature simulation over northern Taiwan

This study evaluates the impact of urbanization over northern Taiwan using the Weather Research and Forecasting (WRF) Model coupled with the Noah land-surface model and a modified urban canopy model (WRF–UCM2D). In the original UCM coupled to WRF (WRF–UCM), when the land use in the model grid is identified as "urban", the urban fraction value is fixed. Similarly, the UCM assumes the distribution of anthropogenic heat (AH) to be constant. This may not only lead to over- or underestimation of urban fraction and AH in urban and non-urban areas, but spatial variation also affects the model-estimated temperature. To overcome the abovementioned limitations and to improve the performance of the original UCM model, WRF–UCM is modified to consider the 2-D urban fraction and AH (WRF–UCM2D). The two models were found to have comparable temperature simulation performance for urban areas, but large differences in simulated results were observed for non-urban areas, especially at nighttime. WRF–UCM2D yielded a higher correlation coefficient (R2) than WRF–UCM (0.72 vs. 0.48, respectively), while bias and RMSE achieved by WRF–UCM2D were both significantly smaller than those attained by WRF–UCM (0.27 and 1.27 vs. 1.12 and 1.89, respectively). In other words, the improved model not only enhanced correlation but also reduced bias and RMSE for the nighttime data of non-urban areas. WRF–UCM2D performed much better than WRF–UCM at non-urban stations with a low urban fraction during nighttime. The improved simulation performance of WRF–UCM2D in non-urban areas is attributed to the energy exchange which enables efficient turbulence mixing at a low urban fraction. The result of this study has a crucial implication for assessing the impacts of urbanization on air quality and regional climate.
Aerosol optical properties derived from the DRAGON-NE Asia campaign, and implications for a single-channel algorithm to retrieve aerosol optical depth in spring from Meteorological Imager (MI) on-board the Communication, Ocean, and Meteorological Satellite (COMS)

An aerosol model optimized for northeast Asia is updated with the inversion data from the Distributed Regional Aerosol Gridded Observation Networks (DRAGON)-northeast (NE) Asia campaign which was conducted during spring from March to May 2012. This updated aerosol model was then applied to a single visible channel algorithm to retrieve aerosol optical depth (AOD) from a Meteorological Imager (MI) on-board the geostationary meteorological satellite, Communication, Ocean, and Meteorological Satellite (COMS). This model plays an important role in retrieving accurate AOD from a single visible channel measurement. For the single-channel retrieval, sensitivity tests showed that perturbations by 4 % (0.926 ± 0.04) in the assumed single scattering albedo (SSA) can result in the retrieval error in AOD by over 20 %. Since the measured reflectance at the top of the atmosphere depends on both AOD and SSA, the overestimation of assumed SSA in the aerosol model leads to an underestimation of AOD. Based on the AErosol RObotic NETwork (AERONET) inversion data sets obtained over East Asia before 2011, seasonally analyzed aerosol optical properties (AOPs) were categorized by SSAs at 675 nm of 0.92 ± 0.035 for spring (March, April, and May). After the DRAGON-NE Asia campaign in 2012, the SSA during spring showed a slight increase to 0.93 ± 0.035. In terms of the volume size distribution, the mode radius of coarse particles was increased from 2.08 ± 0.40 to 2.14 ± 0.40. While the original aerosol model consists of volume size distribution and refractive indices obtained before 2011, the new model is constructed by using a total data set after the DRAGON-NE Asia campaign. The large volume of data in high spatial resolution from this intensive campaign can be used to improve the representative aerosol model for East Asia. Accordingly, the new AOD data sets retrieved from a single-channel algorithm, which uses a precalculated look-up table (LUT) with the new aerosol model, show an improved correlation with the measured AOD during the DRAGON-NE Asia campaign. The correlation between the new AOD and AERONET value shows a regression slope of 1.00, while the comparison of the original AOD data retrieved using the original aerosol model shows a slope of 1.08. The change of y-offset is not significant, and the correlation coefficients for the comparisons of the original and new AOD are 0.87 and 0.85, respectively. The tendency of the original aerosol model to overestimate the retrieved AOD is significantly improved by using the SSA values in addition to size distribution and refractive index obtained using the new model.
Evaluation of the size segregation of elemental carbon (EC) emission in Europe: influence on the simulation of EC long-range transportation

Elemental Carbon (EC) has a significant impact on human health and climate change. In order to evaluate the size segregation of EC emission in the EUCAARI inventory and investigate its influence on the simulation of EC long-range transportation in Europe, we used the fully coupled online Weather Research and Forecasting/Chemistry model (WRF-Chem) at a resolution of 2 km focusing on a region in Germany, in conjunction with a high-resolution EC emission inventory. The ground meteorology conditions, vertical structure and wind pattern were well reproduced by the model. The simulations of particle number and/or mass size distributions were evaluated with observations at the central European background site Melpitz. The fine mode particle concentration was reasonably well simulated, but the coarse mode was substantially overestimated by the model mainly due to the plume with high EC concentration in coarse mode emitted by a nearby point source. The comparisons between simulated EC and Multi-angle Absorption Photometers (MAAP) measurements at Melpitz, Leipzig-TROPOS and Bösel indicated that the coarse mode EC (ECc) emitted from the nearby point sources might be overestimated by a factor of 2–10. The fraction of ECc was overestimated in the emission inventory by about 10–30 % for Russia and 5–10 % for Eastern Europe (e.g., Poland and Belarus). This incorrect size-dependent EC emission results in a shorter atmospheric life time of EC particles and inhibits the long-range transport of EC. A case study showed that this effect caused an underestimation of 20–40 % in the EC mass concentration in Germany under eastern wind pattern.
Drizzle formation in stratocumulus clouds: effects of turbulent mixing

The mechanism of drizzle formation in shallow stratocumulus clouds and the effect of turbulent mixing on this process are investigated. A Lagrangian–Eularian model of the cloud-topped boundary layer is used to simulate the cloud measured during flight RF07 of the DYCOMS-II field experiment. The model contains ~ 2000 air parcels that are advected in a turbulence-like velocity field. In the model all microphysical processes are described for each Lagrangian air volume, and turbulent mixing between the parcels is also taken into account. It was found that the first large drops form in air volumes that are closest to adiabatic and characterized by high humidity, extended residence near cloud top, and maximum values of liquid water content, allowing the formation of drops as a result of efficient collisions. The first large drops form near cloud top and initiate drizzle formation in the cloud. Drizzle is developed only when turbulent mixing of parcels is included in the model. Without mixing, the cloud structure is extremely inhomogeneous and the few large drops that do form in the cloud evaporate during their sedimentation. It was found that turbulent mixing can delay the process of drizzle initiation but is essential for the further development of drizzle in the cloud.
Mid-21st century air quality at the urban scale under the influence of changed climate and emissions – case studies for Paris and Stockholm

Ozone, PM10 and PM2.5 concentrations over Paris, France and Stockholm, Sweden were modelled at 4 and 1 km horizontal resolutions respectively for the present and 2050 periods employing decade-long simulations. We account for large-scale global climate change (RCP-4.5) and fine-resolution bottom-up emission projections developed by local experts and quantify their impact on future pollutant concentrations. Moreover, we identify biases related to the implementation of regional-scale emission projections by comparing modelled pollutant concentrations between the fine- and coarse-scale simulations over the study areas. We show that over urban areas with major regional contribution (e.g. the city of Stockholm) the bias related to coarse-scale projections may be significant and lead to policy misclassification. Our results stress the need to better understand the mechanism of bias propagation across the modelling scales in order to design more successful local-scale strategies. We find that the impact of climate change is spatially homogeneous in both regions, implying strong regional influence. The climate benefit for ozone (daily mean and maximum) is up to −5 % for Paris and −2 % for Stockholm city. The climate benefit on PM2.5 and PM10 in Paris is between −5 and −10 %, while for Stockholm we estimate mixed trends of up to 3 % depending on season and size class. In Stockholm, emission mitigation leads to concentration reductions up to 15 % for daily mean and maximum ozone and 20 % for PM. Through a sensitivity analysis we show that this response is entirely due to changes in emissions at the regional scale. On the contrary, over the city of Paris (VOC-limited photochemical regime), local mitigation of NOx emissions increases future ozone concentrations due to ozone titration inhibition. This competing trend between the respective roles of emission and climate change, results in an increase in 2050 daily mean ozone by 2.5 % in Paris. Climate and not emission change appears to be the most influential factor for maximum ozone concentration over the city of Paris, which may be particularly interesting from a health impact perspective.
Contribution of ship emissions to the concentration and deposition of air pollutants in Europe

Emissions from the marine transport sector are one of the least-regulated anthropogenic emission sources and contribute significantly to air pollution. Although strict limits were introduced recently for the maximum sulfur content in marine fuels in the SECAs (sulfur emission control areas) and in EU ports, sulfur emissions outside the SECAs and emissions of other components in all European maritime areas have continued to increase in the last two decades. We have used the air quality model CAMx (Comprehensive Air Quality Model with Extensions) with and without ship emissions for the year 2006 to determine the effects of international shipping on the annual as well as seasonal concentrations of ozone, primary and secondary components of PM2.5, and the dry and wet deposition of nitrogen and sulfur compounds in Europe. The largest changes in pollutant concentrations due to ship emissions were predicted for summer. Concentrations of particulate sulfate increased due to ship emissions in the Mediterranean (up to 60 %), the English Channel and the North Sea (30–35 %), while increases in particulate nitrate levels were found especially in the north, around the Benelux area (20 %), where there were high NH3 land-based emissions. Our model results showed that not only are the atmospheric concentrations of pollutants affected by ship emissions, but also depositions of nitrogen and sulfur compounds increase significantly along the shipping routes. NOx emissions from the ships, especially in the English Channel and the North Sea, cause a decrease in the dry deposition of reduced nitrogen at source regions by moving it from the gas phase to the particle phase which then contributes to an increase in the wet deposition at coastal areas with higher precipitation. In the western Mediterranean region, on the other hand, model results show an increase in the deposition of oxidized nitrogen (mostly HNO3) due to the ship traffic. Dry deposition of SO2 seems to be significant along the shipping routes, whereas sulfate wet deposition occurs mainly along the Scandinavian and Adriatic coasts. The results presented in this paper suggest that evolution of NOx emissions from ships and land-based NH3 emissions will play a significant role in future European air quality.
Four-year long-path monitoring of ambient aerosol extinction at a central European urban site: dependence on relative humidity

The ambient aerosol particle extinction coefficient is measured with the Spectral Aerosol Extinction Monitoring System (SÆMS) along a 2.84 km horizontal path at 30–50 m height above ground in the urban environment of Leipzig (51.3° N, 12.4° E), Germany, since 2009. The dependence of the particle extinction coefficient (wavelength range from 300 to 1000 nm) on relative humidity up to almost 100 % was investigated. The main results are presented. For the wavelength of 550 nm, the mean extinction enhancement factor was found to be 1.75 ± 0.4 for an increase of relative humidity from 40 to 80 %. The respective 4-year mean extinction enhancement factor is 2.8 ± 0.6 for a relative-humidity increase from 40 to 95 %. A parameterization of the dependency of the urban particle extinction coefficient on relative humidity is presented. A mean hygroscopic exponent of 0.46 for the 2009–2012 period was determined. Based on a backward trajectory cluster analysis, the dependence of several aerosol optical properties for eight air flow regimes was investigated. Large differences were not found, indicating that local pollution sources widely control the aerosol conditions over the urban site. The comparison of the SÆMS extinction coefficient statistics with respective statistics from ambient AERONET sun photometer observations yields good agreement. Also, time series of the particle extinction coefficient computed from in situ-measured dry particle size distributions and humidity-corrected SÆMS extinction values (for 40 % relative humidity) were found in good overall consistency, which verifies the applicability of the developed humidity parameterization scheme. The analysis of the spectral dependence of particle extinction (Ångström exponent) revealed an increase of the 390–881 nm Ångström exponent from, on average, 0.3 (at 30 % relative humidity) to 1.3 (at 95 % relative humidity) for the 4-year period.
High concentrations of sub-3nm clusters and frequent new particle formation observed in the Po Valley, Italy, during the PEGASOS 2012 campaign

The concentrations of neutral and charged sub-3nm clusters and their connection to new particle formation (NPF) were investigated during the PEGASOS campaign (7 June–9 July 2012) at the San Pietro Capofiume measurement station in the Po Valley, Italy. Continuous high concentrations of sub-3nm clusters were detected during the measurement period, although the condensation sink was relatively high (median value 1.1 × 10−2 s−1). The median cluster concentrations were 2140 and 7980 cm−3 in the size bins of 1.5–1.8 and 1.8–3 nm, and the majority of them were electrically neutral. NPF events were observed during the measurement period frequently, on 86 % of the days. The median growth rates of clusters during the events were 4.3, 6.0 and 7.2 nm h−1 in the size ranges of 1.5–3, 3–7 and 7–20 nm. The median formation rate of 1.6 nm clusters was high, 45 cm−3 s−1, and it exceeded the median formation rate of 2 nm clusters by 1 order of magnitude. The ion-induced nucleation fraction was low; the median values were 0.7 % at 1.6 nm and 3.0 % at 2 nm. On NPF event days the neutral cluster concentration had a maximum around 09:00 (local winter time), which was absent on a non-event day. The increase in the cluster concentrations in the morning coincided with the increase in the boundary layer height. At the same time radiation, temperature and SO2 concentration increased, and RH and condensation sink decreased. The concentrations of neutral and charged clusters were observed to have a positive correlation with sulfuric acid proxy, indicating the significance of sulfuric acid for the cluster formation in San Pietro Capofiume. The condensation sink had a negative correlation with the concentration of charged clusters but no clear relation to the neutral cluster concentration. This finding, together with back-trajectory analysis, suggests that the precursor vapors of the clusters and background aerosol particles, acting as their sink, have possibly originated from the same sources, including e.g., power plants and industrial areas in the Po Valley.
Sensitivity of simulated CO2 concentration to sub-annual variations in fossil fuel CO2 emissions

Recent advances in fossil fuel CO2 (FFCO2) emission inventories enable sensitivity tests of simulated atmospheric CO2 concentrations to sub-annual variations in FFCO2 emissions and what this implies for the interpretation of observed CO2. Six experiments are conducted to investigate the potential impact of three cycles of FFCO2 emission variability (diurnal, weekly and monthly) using a global tracer transport model. Results show an annual FFCO2 rectification varying from −1.35 to +0.13 ppm from the combination of all three cycles. This rectification is driven by a large negative diurnal FFCO2 rectification due to the covariation of diurnal FFCO2 emissions and diurnal vertical mixing, as well as a smaller positive seasonal FFCO2 rectification driven by the covariation of monthly FFCO2 emissions and monthly atmospheric transport. The diurnal FFCO2 emissions are responsible for a diurnal FFCO2 concentration amplitude of up to 9.12 ppm at the grid cell scale. Similarly, the monthly FFCO2 emissions are responsible for a simulated seasonal CO2 amplitude of up to 6.11 ppm at the grid cell scale. The impact of the diurnal FFCO2 emissions, when only sampled in the local afternoon, is also important, causing an increase of +1.13 ppmv at the grid cell scale. The simulated CO2 concentration impacts from the diurnally and seasonally varying FFCO2 emissions are centered over large source regions in the Northern Hemisphere, extending to downwind regions. This study demonstrates the influence of sub-annual variations in FFCO2 emissions on simulated CO2 concentration and suggests that inversion studies must take account of these variations in the affected regions.
Ammonia in the summertime Arctic marine boundary layer: sources, sinks, and implications

Continuous hourly measurements of gas-phase ammonia (NH3(g)) were taken from 13 July to 7 August 2014 on a research cruise throughout Baffin Bay and the eastern Canadian Arctic Archipelago. Concentrations ranged from 30 to 650 ng m−3 (40–870 pptv) with the highest values recorded in Lancaster Sound (74°13′ N, 84°00′ W). Simultaneous measurements of total ammonium ([NHx]), pH and temperature in the ocean and in melt ponds were used to compute the compensation point (χ), which is the ambient NH3(g) concentration at which surface–air fluxes change direction. Ambient NH3(g) was usually several orders of magnitude larger than both χocean and χMP (< 0.4–10 ng m3) indicating these surface pools are net sinks of NH3. Flux calculations estimate average net downward fluxes of 1.4 and 1.1 ng m−2 s−1 for the open ocean and melt ponds, respectively. Sufficient NH3(g) was present to neutralize non-sea-salt sulfate (nss-SO42−) in the boundary layer during most of the study. This finding was corroborated with a historical data set of PM2.5 composition from Alert, Nunavut (82°30′ N, 62°20′ W) wherein the median ratio of NH4+/nss-SO42− equivalents was greater than 0.75 in June, July and August. The GEOS-Chem chemical transport model was employed to examine the impact of NH3(g) emissions from seabird guano on boundary-layer composition and nss-SO42− neutralization. A GEOS-Chem simulation without seabird emissions underestimated boundary layer NH3(g) by several orders of magnitude and yielded highly acidic aerosol. A simulation that included seabird NH3 emissions was in better agreement with observations for both NH3(g) concentrations and nss-SO42− neutralization. This is strong evidence that seabird colonies are significant sources of NH3 in the summertime Arctic, and are ubiquitous enough to impact atmospheric composition across the entire Baffin Bay region. Large wildfires in the Northwest Territories were likely an important source of NH3, but their influence was probably limited to the Central Canadian Arctic. Implications of seabird-derived N-deposition to terrestrial and aquatic ecosystems are also discussed.